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MICROPOLLUTANTS IN THE AQUATIC ENVIRONMENT AND THEIR REMOVAL

IN WASTEWATER TREATMENT WORKS
Conference Paper · October 2015
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9th European Waste Water Management Conference
12-13 October 2015, Manchester, UK
MICROPOLLUTANTS IN THE AQUATIC ENVIRONMENT AND THEIR REMOVAL

IN WASTEWATER TREATMENT WORKS
Antakyali, D.1, Morgenschweis, C.2, de Kort, T.2, Sasse, R.1 Schulz, J.1 and Herbst, H.1
1 Grontmij GmbH, Germany, 2 Grontmij B.V., Netherlands
Corresponding Author Email demet.antakyali@grontmij.de
Abstract
Micropollutants are known for their potential to significantly affect the aquatic environment. The
environmental impact of these substances is expressed particularly by their persistency,
bioaccumulation potential and toxicity. Effective test methods regarding their ecological toxicity are
currently under research. Municipal wastewater treatment works (WWTWs) are among the most
important entry paths of micropollutants into surface water bodies. Recent investigations proved that
oxidative and adsorptive methods can be applied cost-effectively for micropollutant removal. Various
removal units have been already implemented in full-scale in municipal WWTWs in Germany,
Switzerland and France. In the Netherlands treatment units including micropollutant removal have
been constructed in hospitals. Further full-scale plants are currently being planned. The paper
presents an overview on the general impacts of micropollutants, effective techniques for their removal
and current implementations in Europe.
Keywords
activated carbon, adsorption, micropollutant removal, ozonation, wastewater treatment
Introduction
The term “micropollutants” basically represents the residues of chemicals occurring in the water-soil-
air matrix in trace amounts from microgram to pictogram per litre and literally underlines the low
concentration range of the substances. Pharmaceuticals, cosmetic products, artificial musk, industrial
auxiliary chemicals, pesticides and biocides are among the substance groups considered as
micropollutants. These are released into the hydrological cycle through urban and agricultural
sources.
The effects of micropollutants in aquatic ecosystem are not very well known yet. However, there are
clear indications for their significant impact potential, particularly considering the long-term impacts.
Reasons for this are (1) their potential to accumulate into aquatic organisms and human bodies
(bioaccumulation), (2) their toxicity and (3) their resistance to degradation in the environment
(persistency). Regulations on their emission and discharge are thus decisive for improving the aquatic
environment and surface water quality.
The Water Framework Directive 2000/60/EC (CEC, 2000) is the European-wide legislation tackling
the hazards and risks arising from priority substances. It aims for good ecological and chemical
conditions in surface water bodies and regulates the monitoring and measures of the EU Member
States towards improving the surface water quality. In 2013, the new Directive 2013/39/EC (CEC,
2013) came into force, amending the Directives 2000/60/EC and 2008/105/EC (CEC, 2008), which
previously amended the Directive 2000/60/EC, as regards to the list of priority substances. More
specifically, twelve new substances were introduced and thus, 45 compounds are now classified as
priority substances. A remarkable number of the substances given in the priority list, particularly
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biocides and industrial auxiliary chemicals are considered as micropollutants due to their nature,
impact and concentration range. There is a waiting list with another 100 substances that will be
assessed for inclusion during the next review process. Regarding the known effects of micropollutants
and the expected future developments such as increased consumption of the chemicals associated
with the demographic rise, intensified actions shall be taken towards minimising the release of
micropollutants into surface water bodies (ARGE KOM-M.NRW, 2015).
The entry pathways of micropollutants into surface water bodies are diverse. Current findings about
the hazardous feature of these chemicals first raise the question whether they can be replaced by
harmless alternatives. This is partly possible and should be a primary goal for the policy makers.
However, it is very unlikely that a full replacement of these chemicals by the harmless ones will be
possible, as certain hazardous features, such as endocrine manipulation (hormonal pharmaceuticals)
or fatal effects (antibiotics, pesticides) are desired effects. Thus to prevent the release of
micropollutants in the aquatic environment, a multi-barrier concept is required. This implies actions
towards preventing micropollutants from entering the hydrological cycle at the source as well as
elimination measures. Regarding the latter, a broad spectrum of micropollutants enter surface water
bodies through municipal wastewater treatment works (WWTWs), making them an important source
for micropollutant release. Thus, advanced wastewater treatment technologies can contribute to the
micropollutant removal significantly.
Micropollutants in surface waters
Wastewater-relevant micropollutants
The number of compounds introduced into the environment by humans is in the thousands (Rosi-
Marshall and Royer, 2012). However, not all of them are relevant for wastewater. Common
micropollutants found in municipal wastewater are discussed in this report as general
pharmaceuticals, endocrine disrupting compounds (EDCs) and biocides. Some sample wastewater-
relevant substances are given in Table 1.
Table 1: Sample micropollutants found in municipal wastewater
Substance Utilisation purpose

Carbamazepine Antiepileptic (pharmaceutical)
Diclofenac Anti-inflammatory (pharmaceutical)
Propyphenazone Analgesic, antipyretic (pharmaceutical)
Caffeine Stimulant (food & pharmaceutical)
AHTN & HHCB Fragrance (personal care product)
Benzophenone Sun blocking crèmes, plastics (industrial auxiliary chemical)
Bisphenol A Basic component for plastics (industrial auxiliary chemical)
TCEP & TCPP & TDCPP Flame retardant (industrial auxiliary chemical)
DEET Insect repellent (biocide)
4-nonylphenoles Industrial surfactant, pesticide (biocide)
Terbutryn Algicide, herbicide (biocide)
2-hydroxybiphenyl Disinfectant, fungicide (biocide)
Pharmaceuticals
The group includes a wide variety of substances, e.g., cardiovascular, antiepileptic, analgesic, and
cytostatic pharmaceuticals, antibiotics, antidepressants, X-ray contrasting agents and sexual
enhancement drugs. The major part of research on pharmaceuticals in the aquatic environment has
focused on occurrence and concentration of the compounds in the surface water, and a number of
studies has investigated the short term effects of individual pharmaceuticals on aquatic organisms
under laboratory conditions and in higher doses. On the way how pharmaceuticals in low
concentrations affect ecosystem functioning, literature is scarce (Rosi-Marshall and Royer, 2012;
STOWA, 2015).
Endocrine disrupting compounds
Endocrine disrupting compounds (EDCs) are a group of substances that exert hormonal activity in
organisms and/or interfere in a different way with the endocrine system in organisms. This group
includes hormone preparations (e.g. synthetic oestrogens like ethinyl estradiol used in birth control
pills), a number of industrial auxiliary chemicals (e.g. perfluorinated compounds like PFOS,
plasticizers like phthalates and Bisphenol-A), organotin compounds (e.g. TBT), pesticides (e.g. DDT),
synthetic fragrances (e.g. musks) and personal care products.
Biocides, including pesticides and disinfectants
This group includes pesticides, disinfectants and anti-fouling agents. Disinfectants are intended to kill
off microorganisms that are present on surfaces. Anti-fouling agents are used on surfaces to prevent
growth of organisms. These are used, for instance, on ship hulls and in piping of cooling water
systems. Pesticides are a wide variety of biologically active substances exterminate in general
specific groups of organisms such as insects (insecticides), algae (algaecides), weeds (herbicides),
fungi (fungicides), etc. Pesticides are mainly used in agriculture, but also to preserve materials in
storage and in the killing of plagues that pose threats to human health.
Ecological effects of common groups of micropollutants
The ecological impact of the micropollutants depends basically on their concentrations, persistence
and the accumulation tendency in living organisms. The impact can be chronic or acute 1 and is to be
expected on individual organisms or community and ecosystem level. In general, chronic effects occur
at lower concentrations than acute effects. Table 2 gives an overview on the known effects.
Substances that have hormone-like behaviour (endocrine disrupting compounds) can cause effects at
very low concentrations, as hormones are messenger agents functioning at low concentration range.
The same holds true for a wide variety of pharmaceuticals that are specifically designed to be
biologically active in target organisms. Persistent compounds – like some pesticides - are known to
accumulate in ecosystems, so even if concentrations in the effluent are relatively low, they may rise
over time. Also, if there is a continuous input of less persistent micropollutants into the aquatic
ecosystem, this may cause negative chronic effects as well, as organisms are continuously exposed
to a certain concentration of (a mixture of) micropollutants.
1
Acute effects are effects that have a direct impact on the organism, like mortality. Chronic effects are more subtle – reduced
reproduction, behavioural changes or feminisation of populations – and show at lower concentrations. Effects on individual level
can have significant effects on population and community level, and hence, on the stability of aquatic ecosystems.
Table 2: Overview on the impact of selected micropollutant groups on living organisms
Group Class Examples of specific effects
- Inhibition of growth of certain (micro)algae in 72 and 96 h experiments

starting at 6 μg/L (Santos et al., 2010; Kümmerer, 2009)
- Effects on nitrification activity (at 9 mg/L) (Klaver and Matthews, 1994)
Antibiotics - Effects on reproduction, hatching and viability of juvenile stages of
crustaceans (e.g. water fleas) at conc. < 1 mg/L (Kümmerer, 2009)
- Secondary effects in crustaceans by alteration of associated microbiota
due to effects of antibiotics (Kümmerer, 2009)
- Effects on activity and behavior (reduced fleeing response) of damselfly

Antihistamines larvae starting at concentrations of 0.4 μg/L, due to neurotransmitter-like
behavior of antihistamines (Jonsson et al., 2014)
- Behavioral changes in fish at environmentally relevant concentrations:

Antidepressants
e.g. aggressive behavior and increased activity in perch exposed to 1.8 μg
Pharmaceuticals
and anti-anxiety
oxazepam/L; impact on mating behavior of fathead minnows starting at
medication
conc. of 1 μg Prozac/L (Brodin et al., 2013; Weinberger and Klaper, 2014)
Anti-inflammatory - Cell damage in trouts after 3-week exposure to concentrations >0.5 μg

drugs diclofenac/L (Mehinto et al., 2010)
- The threshold value for endocrine disrupting effects is ~ 0.5 ng 17a-

ethinylestradiol/L. Effects range from lower egg production in female fish,
(Synthetic)
to growth reduction, increased liver size, feminisation of young male fish to
hormones
overall disruption of the natural hormonal balance. Similar effects occur in
molluscs (ICPR, 2011; STOWA, 2015; Jobling and Tyler, 2003)
- Larval development in certain crustaceans (copepods) is affected at

Endocrine disrupting compounds
Synthetic musk concentrations of 20 μg HHCB/L; at concentrations of 200 20 μg/L,

fragrances proteins involved in excretion of xenobiotic compounds are inhibited
(Walters et al., 2005; Peck and Hornbuckle, 2006).
- Development of male sex organs in female sea snails (imposex) at

Antifoulants concentrations of 1 ng TBT/l and total reproductive failure in sea snails at
concentrations of 6-8 ng TBT/l (Sumpter, 2002).
- Effects of bisphenol-A on egg production in aquatic snails starting at 8

Plasticizers ng/l; effects on reproduction in daphnids starting at 3 to 30 μg DEHP/l
(Jobling et al., 2004; OEHHA, 2009)
Triclosan and triclocarban affect the growth of algae and fresh water
crustaceans from concentrations <0.1 µg/l; decreased aggression (nest
Desinfectants
protection behavior) in Fathead minnows at concentrations of 1.6 μg
triclosan/L (STOWA, 2015; Brausch and Rand, 2011)
Very wide range of effects on target and non-target species, including

acute (e.g., mortality) and chronic effects (reduced reproduction, behavioral
changes, growth inhibition, endocrine disruption). Also higher food chain
Pesticides
effects may occur: decline of farmlandbird populations in the vicinity of
surface waters with imidacloprid concentrations >20 μg/L has been
Biocides
observed in a long-term study (Hallmann et al., 2014).
Antifoulants see antifoulants in the endocrine disrupting compound section
Another possible scenario is incidental input in the surface water of high concentrations of
micropollutants through effluent discharge. In fact, the exposure to a single micropollutant may not
have an effect on the ecosystem, but the combined exposure to numerous micropollutants at low
concentrations may have a negative impact. This may lead to acute effects on the ecosystem, from
which populations and communities need to recuperate. However, if this recuperation takes longer
than time between incidental discharges, or if the impact is too hard to recuperate from, the negative
impacts on the aquatic ecosystem may be long-lasting (EU, 2009; EU, 2012).
Finally, the relevance of micropollutants to a surface water ecosystem also depends on the sensitivity
of the ecosystem and the input of specific compounds or groups of compounds in the system, both in
terms of concentration and duration between inputs. This makes the question of micropollutants also
a location-specific issue.
Determination of the ecological impact of micropollutants
Biological test methods
Ecotoxicological testing in addition to chemical analyses
Chemical analyses of micropollutants give insight in the presence or absence of these compounds in
surface water, waste water and effluent above a compound-specific limit of detection. Therefore, it is a
useful way to look at removal efficiency of micropollutants by WWTWs with or without advanced
techniques. However, this insight is limited to the compounds that are analysed. In some cases, the
metabolites of a micropollutant are more toxic than the initial compound. In chemical analyses this
may not show up.
Translation of concentrations of micropollutants to the effects on organisms is a challenge in itself. In

environmental samples complex mixtures of micropollutants may be present. With the current state of
knowledge on effects of complex mixtures of micropollutants in the aquatic environment, it is hard to
predict whether certain groups of substances add to, enhance or diminish each other’s effect.
Especially persistent (not easily degradable) micropollutants deserve attention, as those may
accumulate in the environment.
Because of aforementioned reasons, ecotoxicological analyses of discharged wastewater (Whole

Effluent Testing) may be a valuable addition to chemical analyses. By an effect-based approach
(bioassays) the effects of all toxic substances in an environmental sample can be investigated.
Bioassays
Exposing well-studied organisms under controlled conditions in a laboratory to (an extract of) waste
water samples, gives insight in the ecotoxicity of the mixture of micropollutants in discharge or surface
water. The effects are a measure for the toxicity of the sample: the lower the concentration at which
negative effects occur, the more toxic the sample. Tests are generally performed with at least three
functional groups of organisms (e.g., algae, crustaceans, insects, bacteria), as each (group of)
organism(s) may react differently to a (mixture of) substance(s). They can be short and focusing on
acute effects (e.g., mortality) or long-term and focusing on chronic effects (e.g. growth, reproduction).
Chronic tests are in general more sensitive than acute tests. Effects in chronic bioassays tend to be at
concentrations one to three orders of magnitude lower. With different solid phase extraction methods
micropollutants in water samples can be preconcentrated. Testing these preconcentrated samples
with acute bioassays is a way to get information on chronic effects in organisms. Table 6 gives an
overview on the biotests applied to determine the micropollutant toxicity.
Table 3: Available bioassays categorized according to the indicator organism
Regular
aquatic Acute Chronic
bioassays*
Algae - 72hrs growth rate and biomass

(e.g., ISO 8692) Algae - 96 hrs growth rate and biomass (e.g.,
Plants
Duckweed - 7 days growth rate and OECD 201)
biomass (e.g., OECD 221)
Daphnids (water fleas) - 48hrs

Daphnids (water fleas) - 21 day survival and
Crustaceans mobilisation and behavior (e.g., ISO
reproduction (e.g., OECD 211)
6341)
Brachionus sp. - 24 hrs survival (e.g., Brachionus sp. - 48 hrs survival and
Rotifers
ASTM E1440) reproduction (e.g., ISO 20666)
Chironomid (non-biting midge) larvae - Chironomid (non-biting midge) larvae - 28 day

Insects 2 or 7 day mobilisation (e.g., OECD survival, development and growth (e.g., RIZA
235) 93.027)
Bioluminescence (Microtox assay) - 30

min bioluminescence inhibition of Vibrio
fisheri (e.g., ISO 11348)
Respiration test - inhibition of
respiration of bacteria from activated
Bacteria -
sludge after 30 min or 3 hrs (e.g.,
OECD 209)
Nitrification test - nitrification inhibition
with bacteria from activated sludge after
4 hrs (e.g., ISO 9509)
Early Life Stage test - 30-35 days larval

hatching, survival, development, behavior
and/or growth (e.g., OECD 210)
Juvenile growth test - 28 days growth,
Fish test - 96hrs survival and behavior
development and behavior (e.g., OECD 215)
in adult fish (e.g., OECD 203)
Fish Life cycle test - hatching success, embryo,
Fish egg test - 48hrs embryonic survival
larval and juvenile development, adult
and development (e.g., OECD 236)
development and reproduction in parent and
first generation - this may include effects of
endocrine disruption (e.g., OECD
ENV/JM/MONO(2008)22)
*focus on fresh water tests and species
Bioassays can also be used to test the efficiency of advanced treatment techniques to eliminate
micropollutants from waste water. By testing the toxicity of effluent from a regular WWTW and
comparing that to the toxicity of effluent from a WWTW using advanced techniques, the removal
efficiency to ecotoxicity can be investigated. The influents of those WWTWs must be similar to make a
relevant comparison.
Certain (chronic) effects do not show up easily in regular ecotoxicity tests. This may be the case for
endocrine disruptors, as the effects of these compounds at low concentrations are subtle and may not
show up during the test time of relatively short bioassays. This would require very costly bioassays
that test the effect on multiple generations. However, with relatively simple in-vitro tests on the cellular
level (e.g., CALUX assays), effects of micropollutants – e.g., endocrine disruption - can be
investigated in (waste) water samples (Table 4). For the testing of removal efficiency of
micropollutants in an effect-based manner, the use of multiple species and effect-analyses is
advisable.
Table 4: Other sample bioassays available for testing of toxicity of micropollutants
Other bioassays Examples of tests
Ames test - induction of DNA damage and mutations to specifically modified

Genotoxicity and bacterial strains (Salmonella or E. coli) (e.g., OECD 471)
mutagenicity umuC test - DNA damage to repair systems of cell of specifically modified
Salmonella strains (e.g., ISO 13829)
Wide range of specific assays, e.g.:

DR CALUX and PAH CALUX - Xenobiotics metabolism / dioxin receptor
activation; ER CALUX - Estrogen signalling; ERα CALUX - Estrogen receptor
α-mediated signalling; ERα-anti CALUX - Repression of estrogen receptor α-
mediated signalling; ERβ CALUX - Estrogen receptor β-mediated signalling;
ERβ-anti CALUX - Repression of estrogen receptor β-mediated signalling; AR
CALUX - Androgen receptor activation; AR-anti CALUX - Repression
androgen receptor activation; PR CALUX - Progesterone receptor-mediated
Calux Assays
signalling; PR-anti CALUX - Repression of progesterone receptor-mediated
signalling; GR CALUX - Glucocorticoid receptor-mediated signalling; P53
CALUX - p53-dependent pathway activation / genotoxicity response; genotox
CALUX - p53-dependent pathway activation; ER stress CALUX - Endoplasmic
reticulum stress response; cytotox CALUX - Repression of constitutive
transcriptional activation
See: http://www.biodetectionsystems.com/products/bioassays/available-
assays.html
The development of high-throughput in-vitro bioassays is ongoing at the moment. In the future, these
will be an instrument to screen (eco)toxicological effects of micropollutants in waste- and surface
water in a relatively inexpensive way.
Ecological field studies
Another way to look at ecological effects of micropollutants, is to look at the ecosystem itself. If shifts
the ecological communities at downstream of the effluent discharge. The advantage of looking at the
ecosystem under natural conditions is to see the actual effects on the system. A recent Dutch study
showed that decline in aquatic invertebrate communities and in farmlandbird populations that depend
on those species, is strongly related to the use of imidacloprid – a neonicotinoid insecticide – in the
studied areas (Hallman et al., 2014). These kinds of studies are long-term studies, but incorporated in
regular monitoring programs of the chemical and ecological status of surface water, give insight in
long-term effects of surface water quality, with effects of micropollutants being a part of that.
The advance of ecotoxicity testing in addition to chemical analysis is that the effect of all
micropollutants and its metabolites present in the eflluent are incorporated.
Comparative assessment of the methods
Each method to determine the impact of the micropollutant has its strengths and weaknesses. Table 5
presents an overview on the advantages and disadvantages of chemical, biological and ecosystem
analyses.
Table 5: Other sample bioassays available for testing of toxicity of micropollutants
Advantages Disadvantages
- Information limited to compounds that

+ Gives information on concentrations of are analysed. No information on
Chemical micropollutants in effluent metabolites
analysis + Relatively inexpensive for the regular - No direct relation with effects on
groups of pollutants ecosystem, especially in cases with
complex mixtures of pollutants
+ Information on the effects of the total

- No direct insight in the specific
amount of bioavailable pollutants in an
Ecotoxicological compound(s) that cause the effect
environmental sample
analysis - Chronic tests may be relatively
+ Insight in the specific group(s) of
expensive
organisms that may be at risk
- It may be difficult to isolate the effects

caused by pollution from effects caused
+ The full scope of the ecosystem is
by other factors such as the suitability of
being investigated: seemingly small
the habitat, the absence or presence of
Ecosystem effects may have significant effects at
certain key species, or water quality
studies other places in the ecosystem
parameters like pH and conductivity
- Site-specific information is gathered,
- Effects may be site-specific and
making site-specific measures possible
therefore may be hard to extrapolate to
other sites
In general, combination of monitoring with different analytical methods (chemical and ecotoxicological)
and monitoring of the ecological quality of the surface water near WWTWs, gives the best insight in
the effect WWTW discharge (including removal of micropollutants) has on the ecosystem. Pilot
studies for Waterboards in the Netherlands look into combinations of all three or two (chemical and
ecotoxicological) methods for monitoring purposes. This effect-based and chemical monitoring can be
used as a prioritization and measures selection tool. The ecological and ecotoxicological monitoring
may give insight in which (parts of) waterbodies may be negatively influenced by micropollutants while
the chemical analyses can point to the substances (and possible sources) at which measures should
be focussed.
Micropollutant entry pathways into surface water bodies
There are different pathways for micropollutants entering surface waters. Figure 1 presents the
common sources and routes of micropollutants into surface water.
Wastewater treatment work effluents constitute a very significant pathway, for containing the
micropollutants which were consumed in build-up areas, mainly pharmaceuticals, personal care
products and household chemicals. In fact, whilst relatively concentrated sources of pharmaceuticals
and hormones originate from hospitals, the majority of the load of these substances is released by
domestic households (STOWA, 2011). Also the residues of industrial chemicals enter the surface
waters through WWTW effluents. Combined sewer overflows as well as surface runoff from urban
areas with separate storm water collection system can transport an important load of micropollutants
such as biocides within a short time.
Stadt Industry Industry

Industrie - Direkteinleiter
Farm Town Krankenhaus
Hospital Pflegeeinrichtung
Health care fac. Industrie -
(indirect discharge) (direct discharge)
Indirekteinleiter
Glyphosat, Amidotrizoate, Bisphenole A,

Carbamazepine,
Mecoprop, Ciprofloxacine, PFT,
Diclofenac,
Cloridazon, Diclofenac, TCPP,
Metoprolol, …
Isopuron, … Antibiotica, … MTBE,…
RÜB
Storm water All common Combined sewer

WWTW Water
substances,
Piroxicam, treatment
…
Natural Water Body
Figure 1: Different pathways of micropollutants entering the environment (WWTP:

wastewater treatment plant)
Agricultural areas constitute another important entry pathway for veterinary pharmaceuticals and
pesticides as a diffuse source, yet rather difficult to control by technical installations. WWTWs present
here a concentrated point source, where a large spectrum of micropollutants can be removed at once.
State of the technology in micropollutant removal
Target group for removal processes
Wastewater relevant micropollutants have been discussed in previous sections. The persistence of
the substances to natural and technical degradation processes varies with their physicochemical
properties. Some of the pharmaceuticals can be removed by > 99 % (e.g. Ibuprofen), where some
other are found in the effluent with almost no change (Carbamazepine). It is stated that conventional
biological treatment plants can remove overall half of the micropollutants (Luo et al., 2014). However,
the other half is sufficient to cause the observed impacts. Thus the focus of the micropollutant removal
processes lies on the substances, which cannot be removed through conventional treatment
processes.
Potential techniques for the cost effective removal of micropollutants
Biological treatment can accomplish more, if optimised for enhanced removal of the micropollutants
through membrane bioreactors, biofiltration systems and coagulation-flocculation (e.g. Luo et al.,
2014). Furthermore, wetlands have the potential to remove micropollutants from wastewater (e.g.
Carranza-Diaz et al., 2014) and there is ongoing research in this field. However, there are already
proven technical processes for efficient micropollutant removal. Figure 2 presents an overview on
these processes, being oxidative, adsorptive and physical methods.
Elimination of micropollutants
oxidative adsorptive physical
Advanced Powdered Granulated

Nano- Reverse
Ozonation Oxidation Activated Activated
filtration Osmosis
Processes Carbon Carbon
Figure 2: Practically tested techniques for the removal of micropollutants; the most cost-
effective methods operating at full scale marked in green
The physical methods are based on filtration processes using membrane technology. With respect to
the small particle size of micropollutants, nanofiltration and reverse osmosis are the most effective
physical techniques using membrane filtration. However, neither nanofiltration nor reverse osmosis
offer cost-effective solutions due to high operating pressures and the associated energy demand.
Oxidative processes can generally offer a significant elimination of micropollutants. Advanced
Oxidation Process (AOP) combines the UV treatment and oxidation processes using hydrogen
peroxide (H2O2) or ozone. The AOP is faster than ozonation alone, however, also less cost-efficient.
Adsorptive processes are known from drinking water treatment and can also remove a remarkable
portion of micropollutants.
It must be stated that there is no particular treatment process to remove all different micropollutants at
once. However, from the present state of the art, the ozonation process and the adsorption by means
of powdered activated carbon (PAC) as well as granulated activated carbon (GAC) are considered as
the cost-effective methods for micropollutant removal for full scale applications (e.g. Hernández-Leal
et al., 2011; Margot et al., 2013; Altmann et al., 2014).
Ozonation
Ozone (O3) is an unstable gas and a very strong oxidant, which quickly decomposes to the more
stable gaseous oxygen (O2). Due to its high reactivity, ozone is capable of oxidizing persistent organic
substances to more easily degradable substances (Barjenbruch et al. 2014). The ozonation is an
already well-established process in the drinking water treatment and is particularly beneficial for
 the reduction of bacteria and viruses, and disinfection,

 the oxidation of the organic and inorganic components of water and
 the elimination of odour and colour.
Ozone oxidizes pollutants either directly or indirectly through the generation of hydroxyl (OH) radicals.
In general, both reaction paths can occur. However, depending on the substance characteristics and
the wastewater composition, one of the two processes will predominate. Further influences may arise
from the reactive conditions such as temperature and pH value (Barjenbruch et al., 2014).
The ozonation process is applied to the effluent of the biological treatment in a separate reaction tank,
where ozone is fed through air diffusers or injector systems. Ozone is not easily transportable and
thus must be produced on-site. In order to prevent the release of excess ozone to the final effluent, an
ozone destruction unit is set at the outflow of the reaction tank. The ozonation step is followed by a
biological post-treatment for the removal of possible breakdown products of the oxidation process,
which may still pose a significant danger for living organisms. Biologically activated filtration systems
or maturation ponds as well as fluid-bed or fixed-bed reactors can be implemented for this purpose.
(ARGE KOM-M.NRW, 2015).
The efficiency of the ozone for micropollutant removal may be reduced by any oxisidable matter in the
wastewater due to competition. Regarding the WWTP effluent, dissolved organic carbon (DOC) is
assumed to be the indicator parameter and thus the ozone dosage is set according to the DOC
concentrations. Also nitrite is recommended to determine, as it can increase the ozone demand in the
wastewater.
Adsorption by activated carbon
In the adsorption process gas or liquid molecules are adhered on a solid surface by electrostatic
interaction. Adsorption by activated carbon implies that the adsorbed compounds are completely
removed from the wastewater. If more than one contaminant is present, hydrophobic substances will
be absorbed by carbon more efficiently and, thus, will be removed in larger quantities than hydrophilic
substances. In particular, activated carbon is appropriate for adsorbing non-polar, organic substances
due to its large specific surface that ranges from 500 to 1500 m 2/g (Barjenbruch et al., 2014).
Activated carbon is produced from natural materials such as wood, coconut shell, peat, lignite,
bituminous coal and petroleum residues. The carbon medium is activated by exposing it to steam and
high temperatures of about 1200 °C. The heating causes cracks, gaps and pores which are
associated with surface increases. In general, two different types of carbon are used: Powdered
activated carbon (PAC) with grain sizes below 0,045 mm and granulated activated carbon (GAC) with
grain sizes in the range of 0,5-4,0 mm (Barjenbruch et al., 2014).
PAC treatment is generally implemented after the biological stage, where it is dosed into the WWTW
effluent in a separate contact tank and separated afterwards again in a settling tank. The sludge from
the settling tank can be recirculated into the contact tank or into the activated sludge tank before
withdrawn from the system for disposal. The fine PAC particles require an additional filtration step
following the settling tank (ARGE KOM-M.NRW, 2015).
In GAC applications, GAC is used as filling material in so called fixed-bed filters. The application can
be rather cost-effective in WWTWs with readily existing flocculation filters, since the filling material in
use can be easily replaced by GAC (ARGE KOM-M.NRW, 2015). Unlike PAC, GAC can be
reactivated for reuse. However, compared to PAC, the filters may need larger space due to the
smaller surface area of GAC.
Important factors for the process selection and design
A functioning WWTW is the prerequisite for an efficient micropollutant removal. Organic matter,
especially particles in the effluent can reduce the efficiency of the micropollutant removal processes or
require a larger dimensioning. Instead of enlarging the micropollutant removal step, it may be less
expensive to improve the conventional treatment process or to install a pre-filtration unit before the
oxidation and adsorption steps.
Wastewater flow and composition can play an important role on the selection of the most suitable
process, thus they should be analysed for each plant individually through a screening. Due to the high
number of chemicals considered as micropollutants, the substance selection for the screening may be
challenging at first sight. Local conditions should be considered for each plant, depending on the
potential micropollutant sources within the WWTW catchment. ARGE KOM-M.NRW (2015) presents a
comparative overview on the substance selection by different professional groups.
Both processes can remove a broad spectrum of substances, yet removing efficiencies of adsorption
and oxidation differ slightly with the substance groups. A comparison of the elimination rates between
ozone oxidation and adsorption by Fahlenkamp et al. (2008) indicates that the removal of oestrogens
such as 17β-Estradiol is very high for both techniques. Carbamazepine (antiepileptic), Diclofenac
(painkiller), Sulfamethoxazole (antibiotic) can be more efficiently eliminated by ozonation than by
PAC, while PAC yields better elimination rates for Nonylphenols, Bisphenol A and musks.
The removal efficiency for both of the processes depends on the retention time of the wastewater in
the reaction tank and the dosage of ozone or activated carbon. In general, higher ozone and PAC
doses or frequent exchange of GAC will increase the removal efficiency. However, the design must be
economically optimised. Thus lab-scale tests are recommended to determine the optimum dosage.
Another important factor, which may help reducing the construction costs, is the availability of any
structures to be used for the micropollutant removal step.
The competence centre for micropollutants suggests that the micropollutant removal step should be
designed to eliminate at least 80 % of the sum of the significant micropollutants (ARGE KOM-M.NRW,
2015).
Implemented removal-sites in Europe
Current state of implementations
An adsorption step in a municipal WWTW has already been constructed in 1992 in southern Germany
(state of BW), which was designed for the removal of colour originated from textile dyes. The first
municipal WWTW extension for a targeted micropollutant removal is located in Bad Sassendorf, in the
NRW state of Germany. The plant has been taken into operation in 2009 following a series of lab and
pilot scale investigations. Today, there are 17 municipal WWTWs running a micropollutant removal
unit in Europe. Figure 3 presents the distribution of the operating units according to the size of the
WWTWs.
5
Number of plants
0
10-40 40-100 100-200 200-500 >500
WWTP Size [1000 x PE]
Figure 3: Number of implemented micropollutant removal units in municipal WWTWs in

Europe according to the size of the WWTW (by June 2015)
Of the 17 municipal WWTWs with a micropollutant removal unit, 14 are located in Germany, two in
France and one in Switzerland. In another Dutch WWTW a special process is applied achieving a
partial removal of micropollutants.
Country Size of WWTW [PE] Process in application Source

Germany (NRW) 30 000 Ozonation KomM.NRW, 2015
Germany (NRW) 50 000 Ozonation and PAC KomM.NRW, 2015
Germany (NRW) 380 000 GAC KomM.NRW, 2015
Germany (BW) 725 000 PAC KomS, 2015
Switzerland 150 000 Ozonation Micropoll, 2014
France 26 000 Ozonation Degremont, 2013
France 15 000 Ozonation Micropoll, 2014
Netherlands 165 000 1-STEP©, GAC (partial) Micropoll, 2014
Table 6 gives an overview on the permanent applications including the size of the WWTW and
implemented process. It is seen that both activated carbon adsorption and ozone oxidation processes
found full-scale applications. Of note is the frequency of PAC plants in the state Baden-Württemberg,
which is to be justified by the existing experience in the region with activated carbon plants
descended from past applications with textile dying wastewater.
Table 6: Permanent implementations for micropollutant removal in municipal WWTWs in

Europe (NRW = North Rhine Westphalia; BW = Baden-Württemberg; PAC = powdered activated
carbon; GAC = granulated activated carbon; MBR = membrane bioreactor)
Country Size of WWTW [PE] Process in application Source

Germany (NRW) 50 000 Ozonation and PAC KomM.NRW, 2015

Switzerland 150 000 Ozonation Micropoll, 2014
France 26 000 Ozonation Degremont, 2013
France 15 000 Ozonation Micropoll, 2014
Netherlands 165 000 1-STEP©, GAC (partial) Micropoll, 2014
The tendency for new constructions of micropollutant removal steps in WWTWs is ongoing in central
Europe, in particular in Germany and Switzerland. In Germany micropollutant removal steps are in the
construction or design phase at more than 10 WWTWs. Also in Switzerland the extension of several
other WWTWs with micropollutant removal has been initiated as a consequence of the introduction of
the legal enforcement. One plant is in operation since 2014, and a second one is about to be taken
into full operation. The selection of plants to be extended is based on the WWTW size and feature or
the sensitivity of the receiving water body.
Besides the applications in municipal WWTWs, decentralized plants have been implemented in
several hospitals for hospital wastewater being a hot-spot for pharmaceutical residues. Table 7
presents the basic features of the plants in operation.
Table 7: Permanent decentralised WWTWs including a micropollutant removal step in

hospitals in Europe.
Country Capacity Process in application Source

Germany (NRW) 340 beds, 32 m³/h MBR and Ozonation KomM.NRW 2015
Germany (NRW) 560 beds, 25 m³/h MBR, Ozonation and PAC PILLS 2009
Netherlands 200 beds, 10 m³/h MBR, Ozonation and GAC E. Koetse (Pharmafilter) 2014
(personal communication)
Netherlands 400 beds, 10 m³/h MBR, Ozonation and GAC E. Koetse (Pharmafilter) 2014
(personal communication)
Denmark 900 beds, 15 m³/h MBR, Ozonation and GAC Nielsen et al. 2013
Two plants in Germany, two in Netherlands and one in Denmark are known to the authors. Two more
plants are currently under construction in the Netherlands. The common feature of the implemented
hospital plants is that the plants combine the biological wastewater treatment with a post-treatment
micropollutant removal step in decentralized units.
Cost of the micropollutant removal step
The costs associated with micropollutant treatment will vary dependent upon the availability of existing
assets, the substances to be removed and the flow to be treated. Figure 4 summarises the specific
costs of the implemented plants in Germany and Switzerland (by March 2015).
0,25
0,20
[€/m³treated wastewater]
Specific annual net costs
0,15
0,10
0,05
-
5.000 50.000 500.000
Connected population equivalent [PE]
Figure 4: Specific costs of ozonation and activated carbon processes for different
WWTPs in Germany and Switzerland (source: KOM-M.NRW)
In line with the expectations, larger plants result in the lower specific costs. No clear cost advantage
between PAC, GAC or ozone can be observed. The data contains plants, where existing structures
have been used and also those only with new installations. Thus an exact cost comparison is not
possible. However, a general tendency around 10 Euro cents per m³ treated wastewater can be
recognised.
Conclusions
Types, entry pathways and impact of the micropollutants were discussed. Typical substances
released by municipal wastewater treatment works (WWTW) were presented. Biological test methods
to determine the toxicity of micropollutants were demonstrated. Technical measures to remove the
micropollutants from wastewater were explained and some details on the process selection and
design were given. Finally the state of the full scale implementations in Europe for micropollutant
removal in WWTWs was displayed.
Micropollutants such as pharmaceutical residuals, biocides, industrial auxiliary chemicals, hormones

etc. are likely to have a significant impact on the aquatic environment due to their bioaccumulation
potential, toxicity and persistency. For preventing the entry of micropollutants into surface water
bodies, a multi-barrier concept is needed. Municipal wastewater treatment works (WWTWs) are
among the most important entry pathways for micropollutants into the aquatic environment. As point
sources they technically enable actions to prevent the micropollutant release. Thus they can act as an
important component of a multi-barrier concept.
A significant rejection of micropollutants can be accomplished in WWTWs through the extension with
ozonation or activated carbon adsorption. These techniques are applied subsequent to the
conventional biological treatment step (includes final sedimentation tank). Both techniques can
achieve good results, yet their efficiency on different group of substances can be variable. Oxidation
requires a biological post-treatment process to remove any breakdown products. Considering
micropollutant removal by means of adsorption, both granulated activated carbon (GAC) and
powdered activated carbon (PAC) can be used. PAC step should be finalised by an additional
filtration to reject the very fine carbon particles. The adsorption via GAC is particularly suitable for
WWTWs which already have a filtration system. The design of the plants should consider the
wastewater characteristics and the vulnerability of the receiving water bodies. A preliminary screening
of the incoming wastewater should be conducted prior to the design of a micropollutant removal step.
The costs associated with micropollutant treatment will vary dependent upon the availability of existing
assets, the substances to be removed and the flow to be treated.
Current research focuses on the determination of the efficiency of micropollutant removal and on the
cost-efficient combination of different processes for an optimised process design.
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MICROPOLLUTANTS IN THE AQUATIC ENVIRONMENT AND THEIR REMOVAL

Conference Paper · October 2015

Demet Antakyali Christa Morgenschweis

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MICROPOLLUTANTS IN THE AQUATIC ENVIRONMENT AND THEIR REMOVAL

Corresponding Author Email demet.antakyali@grontmij.de

activated carbon, adsorption, micropollutant removal, ozonation, wastewater treatment

Micropollutants in surface waters

Table 1: Sample micropollutants found in municipal wastewater

Substance Utilisation purpose

Endocrine disrupting compounds

Biocides, including pesticides and disinfectants

Ecological effects of common groups of micropollutants

Table 2: Overview on the impact of selected micropollutant groups on living organisms

Group Class Examples of specific effects

- Inhibition of growth of certain (micro)algae in 72 and 96 h experiments

- Effects on activity and behavior (reduced fleeing response) of damselfly

- Behavioral changes in fish at environmentally relevant concentrations:

Anti-inflammatory - Cell damage in trouts after 3-week exposure to concentrations >0.5 μg

- The threshold value for endocrine disrupting effects is ~ 0.5 ng 17a-

- Larval development in certain crustaceans (copepods) is affected at

Synthetic musk concentrations of 20 μg HHCB/L; at concentrations of 200 20 μg/L,

- Development of male sex organs in female sea snails (imposex) at

- Effects of bisphenol-A on egg production in aquatic snails starting at 8

Very wide range of effects on target and non-target species, including

observed in a long-term study (Hallmann et al., 2014).

Antifoulants see antifoulants in the endocrine disrupting compound section

Determination of the ecological impact of micropollutants

Biological test methods

Ecotoxicological testing in addition to chemical analyses

Translation of concentrations of micropollutants to the effects on organisms is a challenge in itself. In

Because of aforementioned reasons, ecotoxicological analyses of discharged wastewater (Whole

Table 3: Available bioassays categorized according to the indicator organism

Algae - 72hrs growth rate and biomass

Daphnids (water fleas) - 48hrs

Chironomid (non-biting midge) larvae - Chironomid (non-biting midge) larvae - 28 day

Bioluminescence (Microtox assay) - 30

Early Life Stage test - 30-35 days larval

*focus on fresh water tests and species

Table 4: Other sample bioassays available for testing of toxicity of micropollutants

Other bioassays Examples of tests

Ames test - induction of DNA damage and mutations to specifically modified

Wide range of specific assays, e.g.:

Ecological field studies

Comparative assessment of the methods

Table 5: Other sample bioassays available for testing of toxicity of micropollutants

- Information limited to compounds that

+ Information on the effects of the total

- It may be difficult to isolate the effects

Micropollutant entry pathways into surface water bodies

Stadt Industry Industry

Glyphosat, Amidotrizoate, Bisphenole A,

Storm water All common Combined sewer

Natural Water Body

Figure 1: Different pathways of micropollutants entering the environment (WWTP:

State of the technology in micropollutant removal

Target group for removal processes

Potential techniques for the cost effective removal of micropollutants

oxidative adsorptive physical